Liu Yawen, Liu Lina, Diao Xungang, Liang Jie, Wu Chunfei, Sun Yifei
School of Physics, Beihang University, Beijing 100191, China.
College of Environmental Science and Engineering, Nankai University, Tianjing 300350, China.
Waste Manag. 2022 Jun 15;147:1-9. doi: 10.1016/j.wasman.2022.05.007. Epub 2022 May 17.
Ni-modified ZSM-5 catalysts are prepared by a one-pot hydrothermal synthesis method and applied to the steam reforming of naphthalene as a tar model compound. The effects of the reaction temperature, silica-alumina ratio (Si/Al) and metal content on the catalytic performance for reforming naphthalene are investigated. Characterization results indicate that the Ni-modified ZSM-5 catalysts maintain the original MFI structure of ZSM-5 and a portion of Ni is successfully introduced into the zeolite structure. When the reaction temperature is 800 °C, the conversion efficiency of naphthalene achieves 91.5% with a high yield (6.75%) of hydrogen. Zeolite catalysts with higher Si/Al ratios improve the conversion of naphthalene to syngas, demonstrating their better catalytic activity. An appropriate active metal content (2.4 wt%) contributes to the catalytic performance of the catalyst owing to the strong metal-support interaction, resulting in resistance to sintering and carbon deposition. The reaction mechanism involved in the catalytic reforming of naphthalene is proposed. The application of a novel one-pot hydrothermal synthesis method greatly promoted the catalytic activity of Ni@ZSM-5, which provided an appropriate and universal approach for the improvement and optimization of tar reforming catalysts.
采用一锅水热合成法制备了镍改性ZSM-5催化剂,并将其应用于萘作为焦油模型化合物的蒸汽重整反应。研究了反应温度、硅铝比(Si/Al)和金属含量对萘重整催化性能的影响。表征结果表明,镍改性ZSM-5催化剂保持了ZSM-5原有的MFI结构,且部分镍成功引入到沸石结构中。当反应温度为800℃时,萘的转化效率达到91.5%且氢气产率较高(6.75%)。具有较高Si/Al比的沸石催化剂提高了萘转化为合成气的转化率,表明其具有更好的催化活性。由于强金属-载体相互作用,合适的活性金属含量(2.4 wt%)有助于催化剂的催化性能,从而提高其抗烧结和抗积碳性能。提出了萘催化重整的反应机理。新型一锅水热合成法的应用极大地提高了Ni@ZSM-5的催化活性,为焦油重整催化剂的改进和优化提供了一种合适且通用的方法。